Uncertainty quantification (UQ) in natural language generation (NLG) tasks remains an open challenge, exacerbated by the intricate nature of the recent large language models (LLMs). This study investigates adapting conformal prediction (CP), which can convert any heuristic measure of uncertainty into rigorous theoretical guarantees by constructing prediction sets, for black-box LLMs in open-ended NLG tasks. We propose a sampling-based uncertainty measure leveraging self-consistency and develop a conformal uncertainty criterion by integrating the uncertainty condition aligned with correctness into the design of the CP algorithm. Experimental results indicate that our uncertainty measure generally surpasses prior state-of-the-art methods. Furthermore, we calibrate the prediction sets within the model's unfixed answer distribution and achieve strict control over the correctness coverage rate across 6 LLMs on 4 free-form NLG datasets, spanning general-purpose and medical domains, while the small average set size further highlights the efficiency of our method in providing trustworthy guarantees for practical open-ended NLG applications.